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The K- and Co-doped BaFe(2)As(2) (Ba-122) superconducting compounds are potentially useful for applications because they have upper critical fields (H(c2)) of well over 50 T, H(c2) anisotropy γ < 2and thin-film critical current densities J(c) exceeding 1 MA cm(-2) (refs 1-4) at 4.2 K. However, thin-film bicrystals of Co-doped Ba-122 clearly exhibit weak link behaviour for [001] tilt misorientations of more than about 5°, suggesting that textured substrates would be needed for applications, as in the cuprates. Here we present a contrary and very much more positive result in which untextured polycrystalline (Ba(0.6)K(0.4))Fe(2)As(2) bulks and round wires with high grain boundary density have transport critical current densities well over 0.1 MA cm(-2) (self-field, 4.2 K), more than 10 times higher than that of any other round untextured ferropnictide wire and 4-5 times higher than the best textured flat wire. The enhanced grain connectivity is ascribed to their much improved phase purity and to the enhanced vortex stiffness of this low-anisotropy compound (γ~1-2) when compared with YBa(2)Cu(3)O(7-x) (γ~5).

Understanding new superconductors requires high-quality epitaxial thin films to explore intrinsic electromagnetic properties and evaluate device applications. So far, superconducting properties of ferropnictide thin films seem compromised by imperfect epitaxial growth and poor connectivity of the superconducting phase. Here we report new template engineering using single-crystal intermediate layers of (001) SrTiO(3) and BaTiO(3) grown on various perovskite substrates that enables genuine epitaxial films of Co-doped BaFe(2)As(2) with a high transition temperature (T(c,rho=0) of 21.5 K, where rho=resistivity), a small transition width (DeltaT(c)=1.3 K), a superior critical current density J(c) of 4.5 MA cm(-2) (4.2 K) and strong c-axis flux pinning. Implementing SrTiO(3) or BaTiO(3) templates to match the alkaline-earth layer in the Ba-122 with the alkaline-earth/oxygen layer in the templates opens new avenues for epitaxial growth of ferropnictides on multifunctional single-crystal substrates. Beyond superconductors, it provides a framework for growing heteroepitaxial intermetallic compounds on various substrates by matching interfacial layers between templates and thin-film overlayers.